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A Million Turnover Molecular Anode for Catalytic Water Oxidation
Author(s) -
Creus Jordi,
Matheu Roc,
Peñafiel Itziar,
Moonshiram Dooshaye,
Blondeau Pascal,
BenetBuchholz Jordi,
GarcíaAntón Jordi,
Sala Xavier,
Godard Cyril,
Llobet Antoni
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201609167
Subject(s) - catalysis , ruthenium , chemistry , turnover number , pyrene , electrochemistry , terpyridine , x ray absorption spectroscopy , pyridine , anode , inorganic chemistry , metal , medicinal chemistry , electrode , organic chemistry , absorption spectroscopy , physics , quantum mechanics
Molecular ruthenium‐based water oxidation catalyst precursors of general formula [Ru(tda)(L i ) 2 ] (tda 2− is [2,2′:6′,2′′‐terpyridine]‐6,6′′‐dicarboxylato; L 1 =4‐(pyren‐1‐yl)‐ N ‐(pyridin‐4‐ylmethyl)butanamide, 1 b ; L 2 =4‐(pyren‐1‐yl)pyridine), 1 c ), have been prepared and thoroughly characterized. Both complexes contain a pyrene group allowing ready and efficiently anchoring via π interactions on multi‐walled carbon nanotubes (MWCNT). These hybrid solid state materials are exceptionally stable molecular water‐oxidation anodes capable of carrying out more than a million turnover numbers (TNs) at pH 7 with an E app =1.45 V vs. NHE without any sign of degradation. XAS spectroscopy analysis before, during, and after catalysis together with electrochemical techniques allow their unprecedented oxidative ruggedness to be monitored and verified.